Abstract Traditional industrial system integrating denitration and filtration faces the challenge of interfacial instability and the incompatibility between high catalytic performance and low pressure drop. To resolve this dilemma, we construct a novel and efficient catalytic membrane material with a ternary “zeolite catalyst‐coupling agent‐fiber” interfacial synergy, achieving simultaneous air filtration and selective catalytic reduction of NO with NH 3 (NH 3 ‐SCR). The Cu‐SSZ‐13 zeolite catalyst is covalently grafted onto electrospun polyimide fibers through KH550‐induced in situ Si‐O‐Si bonding, forming molecular bridges that stabilize organic‐inorganic interfaces. Response surface methodology optimization yields a membrane with triple functionality: superior low‐temperature NH 3 ‐SCR activity (25 °C window reduction), exceptional filtration efficiency (> 99.99% for PM0.3), and robust industrial adaptability (< 1000 Pa pressure drop). Mechanistic studies reveal dual‐path enhancement: KH550 diversifies nitrate intermediates via Lewis acid enrichment (16.5% activation energy reduction), while the 3D fibrous network reduces boundary layer thickness via CFD‐proven airflow disturbance, accelerating mass transfer. Concurrently, zeolite‐derived nanotextured surfaces enhance particle interception through roughness‐amplified capture mechanisms. This micro‐to‐macro design paradigm creates synergistic “1 + 1 > 2” effects, enabling unprecedented integration of catalytic and filtration functionalities in a single material for industrial flue gas and diesel exhaust purification.